Despite the widespread use of integrated hydrology models in a variety of applications, consideration of multicomponent reactive transport is still not common. The implementation of these processes requires coupling transport at the surface-subsurface interface and efficient solution of the non-linear geochemical model that is consistent with the integrated hydrology solution. The Advanced Terrestrial Simulator provides a flexible multiphysics framework that facilitated this process. In this work, the integrated reactive transport process kernel (PK) was weakly coupled to the integrated hydrology PK. In turn, integrated transport and reactions were coupled using an operator splitting approach. This splitting enabled an explicit solution of the integrated transport problem, including a novel algorithm to calculate exchange fluxes across the surface-subsurface interface and a point-by-point solution of the geochemical problem. Geochemical capabilities were added using well-established external codes, but rather than using a custom interface to each, a generic interface was used that clearly specifies the variables and operations used by the chemistry PK. The implementation is demonstrated with two example simulations: transport of a tracer in a soil column as it saturates over time and water ponds on the surface and reactive transport in a hillslope driven by successive wet-dry cycles that result in infiltration, runoff and exfiltration processes.

Climate change and other disturbances significantly impact hydrogeochemical exports from mountainous headwater catchments such as the Upper Colorado River Basin. Developing a mechanistic understanding of how the physical and chemical processes interact in time and space in an integrated manner is key to quantifying the future impacts of such disturbances. The hydrogeochemical response of a mountainous catchment in the 2010–2019 period is evaluated quantitatively using a high-resolution model that simulates integrated hydrology, and transport and reactions for selected solutes and minerals. The model assumes that pyrite is present only at depth while calcite is distributed uniformly, and captures the observed C-Q reasonably well. Distinct C-Q dynamics are observed in an average (WY16), a wet (WY17), and a dry (WY18) water year. The model also quantifies the water fraction from surface, shallow and deep groundwater compartments using tracers, and suggests greater groundwater contributions to peak stream discharge in the dry WY18. Results demonstrate that calcium concentrations do not change significantly from year to year, while sulfate shows significant temporal variability. Pyrite dissolution is affected by the changing hydrological drivers where it is enhanced in the dry WY18; calcite dissolution supplements calcium dilution under high flow conditions. The model simulates the reaction hotspots controlled by hydrological conditions, and the spatially-resolved results show that higher soil saturation and less snowpack occur earlier on the south-facing side than on the north-facing side. This is a first-of-its-kind demonstration of a model that integrates hydrologic processes, including evapotranspiration, and reactive transport to enable a predictive understanding of hydrogeochemical exports.

A wavelet-based local mesh refinement (wLMR) strategy is designed to generate multiresolution and unstructured triangular meshes from real digital elevation model (DEM) data for efficient hydrological simulations at the catchment scale. The wLMR strategy is studied considering slope- and curvature-based refinement criteria to analyze DEM inputs: the slope-based criterion uses bed elevation data as input to the wLMR strategy, whereas the curvature-based criterion feeds the bed slope data into it. The performance of the wLMR meshes generated by these two criteria is compared for hydrological simulations; first, using three analytical tests with the systematic variation in topography types and then by reproducing laboratory- and real-scale case studies. The bed elevation on the wLMR meshes and their simulation results are compared relative to those achieved on the finest uniform mesh. Analytical tests show that the slope- and curvature-based criteria are equally effective with the wLMR strategy, and that it is easier to decide which criterion to take in relation to the (regular) shape of the topography. For the realistic case studies: (i) slope analysis provides a better metric to assess the correlation of a wLMR mesh to the fine uniform mesh and (ii) both criteria predict outlet hydrographs with a close predictive accuracy to that on the uniform mesh, but the curvature-based criterion is found to slightly better capture the channeling patterns of real DEM data.

Climate resilience is an emerging issue at contaminated sites and hazardous waste sites, since projected climate shifts (e.g., increased/decreased precipitation) and extreme events (e.g., flooding, drought) could affect ongoing remediation or closure strategies. In this study, we develop a reactive transport model (Amanzi) for radionuclides (uranium, tritium, and others) and evaluate how different scenarios under climate change will influence the contaminant plume conditions and groundwater well concentrations. We demonstrate our approach using a two-dimensional (2D) reactive transport model for the Savannah River Site F-Area, including mineral reaction and sorption processes. Different recharge scenarios are considered by perturbing the infiltration rate from the base case as well as considering cap-failure and climate projection scenarios. We also evaluate the uranium and nitrate concentration ratios between scenarios and the base case to isolate the sorption effects with changing recharge rates. The modeling results indicate that the competing effects of dilution and remobilization significantly influence pH, thus changing the sorption of uranium. At the maximum concentration on the breakthrough curve, higher aqueous uranium concentration implies that sorption is reduced with lower pH due to remobilization. To better evaluate the climate change impacts in the future, we develop the workflow to include the downscaled CMIP5 (Coupled Model Intercomparison Project) climate projection data in the reactive transport model and evaluate how residual contamination evolves through 2100 under four climate Representative Concentration Pathway (RCP) scenarios. The integration of climate modeling data and hydrogeochemistry models enables us to quantify the climate change impacts, assess which impacts need to be planned for, and therefore assist climate resiliency efforts and help guide site management.

To understand how redox processes influence carbon, nitrogen, and iron cycling within the intrameander hyporheic zone, we developed a biotic and abiotic reaction network and incorporated it into the reactive transport simulator PFLOTRAN. Two-dimensional reactive flow and transport simulations were performed (1) to evaluate how transient hydrological conditions control the lateral redox zonation within an intrameander region of the East River in Colorado and (2) to quantify the impact of a single meander on subsurface exports of carbon and other geochemical species to the river. The meander's overall contribution to the river was quantified by integrating geochemical outfluxes along the outside of the meander bend. The model was able to capture the field-observed trends of dissolved oxygen, nitrate, iron, pH, and total inorganic carbon along a 2-D transect. Consistent with field observations, simulated dissolved oxygen and nitrate decreased along the intrameander flow paths while iron (Fe2+) concentration increased. The simulation results further demonstrated that the reductive potential of the lateral redox zonation was controlled by groundwater velocities resulting from river stage fluctuations, with low-water conditions promoting reducing conditions. The sensitivity analysis results showed that permeability had a more significant impact on biogeochemical zonation compared to the reaction pathways under transient hydrologic conditions. The simulation results further indicated that the meander acted as a sink for organic and inorganic carbon as well as iron during the extended baseflow and high-water conditions; however, these geochemical species were released into the river during the falling limb of the hydrograph.

Computational and data-enabled science and engineering are revolutionizing advances throughout science and society, at all scales of computing. For example, teams in the U.S. Department of Energy's Exascale Computing Project have been tackling new frontiers in modeling, simulation, and analysis by exploiting unprecedented exascale computing capabilities-building an advanced software ecosystem that supports next-generation applications and addresses disruptive changes in computer architectures. However, concerns are growing about the productivity of the developers of scientific software. Members of the Interoperable Design of Extreme-scale Application Software project serve as catalysts to address these challenges through fostering software communities, incubating and curating methodologies and resources, and disseminating knowledge to advance developer productivity and software sustainability. This article discusses how these synergistic activities are advancing scientific discovery-mitigating technical risks by building a firmer foundation for reproducible, sustainable science at all scales of computing, from laptops to clusters to exascale and beyond.